The absorption‐based optical activities (OA) of chiral inorganic materials without the assistance from organic molecules are limited in the plasmon of chiral metallic nanomaterials and the electron transition of chiral semiconductors at the ultraviolet–visible (UV–vis) region. In this work, chiral mesostructured manganese carbonate (CMMC) nano‐dumbbells with hierarchically chiral structures are synthesized, exhibiting vibrational circular dichroism (VCD) signals. CMMC powders are synthesized by a chiral‐molecule‐induced hydrothermal method. Three levels of hierarchical chirality exist in the CMMC, including primary twisted nanoflakes with distorted crystal lattices at the atomic level, secondary stacking of nanoflakes to form a nanoplate, and tertiary arranged nanoplates to form a twisting nano‐dumbbell. Antipodal CMMC samples exhibit antipodal VCD signals at the infrared region (IR) absorption 1400 and 860 cm–1, attributed to vibrational transitions in the asymmetric electric field and selective light harvesting in the hierarchically chiral structures.